Contribution of the nuclear field shift to kinetic uranium isotope fractionation

Research output: Contribution to journal › Article › Research › peer review

Authors

  • A. R. Brown
  • Yvonne Röbbert
  • A. Sato
  • M. Hada
  • M. Abe
  • R. Bernier-Latmani

Research Organisations

External Research Organisations

  • Hiroshima University
  • École polytechnique fédérale de Lausanne (EPFL)
  • Tokyo Metropolitan University
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Details

Original languageEnglish
Pages (from-to)43-47
Number of pages5
JournalGeochemical Perspectives Letters
Volume27
Early online date9 Oct 2023
Publication statusPublished - 2023

Abstract

Isotopic fractionation of heavy elements (e.g., >100 amu) often invokes the nuclear field shift effect, which is due to the impact of the elements’ large nuclei on electron density. In particular, it has been explicitly described for uranium (U) at equilibrium and during kinetic isotope fractionation in abiotic mercury reactions. By following the fractionation of 233U, 235U, 236U and 238U during the enzymatic reduction of hexavalent U to tetravalent U by the bacterium Shewanella oneidensis, we provide the first direct evidence of the nuclear field shift effect during biologically controlled kinetic isotope fractionation. Here, we observed the odd-even staggering trend between fractionation factors of each isotope and their nuclear masses, and show that fractionation factors are correlated better with the nuclear volume than the mass. Additionally, by computing the relative contributions of the conventional mass-dependent effect (vibrational energy) and the mass-independent effect (nuclear field shift), we demonstrate that the experimental nuclear field shift effect is smaller than the calculated equilibrium value and that this discrepancy is responsible for the kinetic fractionation factor being lower than that predicted at equilibrium.

ASJC Scopus subject areas

Cite this

Contribution of the nuclear field shift to kinetic uranium isotope fractionation. / Brown, A. R.; Röbbert, Yvonne; Sato, A. et al.
In: Geochemical Perspectives Letters, Vol. 27, 2023, p. 43-47.

Research output: Contribution to journal › Article › Research › peer review

Brown, AR, Röbbert, Y, Sato, A, Hada, M, Abe, M & Bernier-Latmani, R 2023, 'Contribution of the nuclear field shift to kinetic uranium isotope fractionation', Geochemical Perspectives Letters, vol. 27, pp. 43-47. https://doi.org/10.7185/GEOCHEMLET.2333
Brown, A. R., Röbbert, Y., Sato, A., Hada, M., Abe, M., & Bernier-Latmani, R. (2023). Contribution of the nuclear field shift to kinetic uranium isotope fractionation. Geochemical Perspectives Letters, 27, 43-47. https://doi.org/10.7185/GEOCHEMLET.2333
Brown AR, Röbbert Y, Sato A, Hada M, Abe M, Bernier-Latmani R. Contribution of the nuclear field shift to kinetic uranium isotope fractionation. Geochemical Perspectives Letters. 2023;27:43-47. Epub 2023 Oct 9. doi: 10.7185/GEOCHEMLET.2333
Brown, A. R. ; Röbbert, Yvonne ; Sato, A. et al. / Contribution of the nuclear field shift to kinetic uranium isotope fractionation. In: Geochemical Perspectives Letters. 2023 ; Vol. 27. pp. 43-47.
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AU - Brown, A. R.

AU - Röbbert, Yvonne

AU - Sato, A.

AU - Hada, M.

AU - Abe, M.

AU - Bernier-Latmani, R.

N1 - Publisher Copyright: © 2023 European Association of Geochemistry. All rights reserved.

PY - 2023

Y1 - 2023

N2 - Isotopic fractionation of heavy elements (e.g., >100 amu) often invokes the nuclear field shift effect, which is due to the impact of the elements’ large nuclei on electron density. In particular, it has been explicitly described for uranium (U) at equilibrium and during kinetic isotope fractionation in abiotic mercury reactions. By following the fractionation of 233U, 235U, 236U and 238U during the enzymatic reduction of hexavalent U to tetravalent U by the bacterium Shewanella oneidensis, we provide the first direct evidence of the nuclear field shift effect during biologically controlled kinetic isotope fractionation. Here, we observed the odd-even staggering trend between fractionation factors of each isotope and their nuclear masses, and show that fractionation factors are correlated better with the nuclear volume than the mass. Additionally, by computing the relative contributions of the conventional mass-dependent effect (vibrational energy) and the mass-independent effect (nuclear field shift), we demonstrate that the experimental nuclear field shift effect is smaller than the calculated equilibrium value and that this discrepancy is responsible for the kinetic fractionation factor being lower than that predicted at equilibrium.

AB - Isotopic fractionation of heavy elements (e.g., >100 amu) often invokes the nuclear field shift effect, which is due to the impact of the elements’ large nuclei on electron density. In particular, it has been explicitly described for uranium (U) at equilibrium and during kinetic isotope fractionation in abiotic mercury reactions. By following the fractionation of 233U, 235U, 236U and 238U during the enzymatic reduction of hexavalent U to tetravalent U by the bacterium Shewanella oneidensis, we provide the first direct evidence of the nuclear field shift effect during biologically controlled kinetic isotope fractionation. Here, we observed the odd-even staggering trend between fractionation factors of each isotope and their nuclear masses, and show that fractionation factors are correlated better with the nuclear volume than the mass. Additionally, by computing the relative contributions of the conventional mass-dependent effect (vibrational energy) and the mass-independent effect (nuclear field shift), we demonstrate that the experimental nuclear field shift effect is smaller than the calculated equilibrium value and that this discrepancy is responsible for the kinetic fractionation factor being lower than that predicted at equilibrium.

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JO - Geochemical Perspectives Letters

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